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Modeling the Frozen-In Anticyclone in the 2005 Arctic Summer Stratosphere

Immediately following the breakup of the 2005 Arctic spring stratospheric vortex, a tropical air mass, characterized by low potential vorticity (PV) and high nitrous oxide (N2O), was advected poleward and became trapped in the easterly summer polar vortex. This feature, known as a "Frozen-In Anticyclone (FrIAC)", was observed in Earth Observing System (EOS) Aura Microwave Limb Sounder (MLS) data to span the potential temperature range from ~580 to 1100 K (~25 to 40 km altitude) and to persist from late March to late August 2005. This study compares MLS N2O observations with simulations from the Global Modeling Initiative (GMI) chemistry and transport model, the GEOS-5/MERRA Replay model, and the Van Leer Icosahedral Triangular Advection (VITA) isentropic transport model to elucidate the processes involved in the lifecycle of the FrIAC, which is here divided into three distinct phases. During the "spin-up phase" (March to early April), strong poleward flow resulted in a tight isolated anticyclonic vortex at ~70–90° N, marked with elevated N2O. GMI, Replay, and VITA all reliably simulated the spin-up of the FrIAC, although the GMI and Replay peak N2O values were too low. The FrIAC became trapped in the developing summer easterly flow and circulated around the polar region during the "anticyclonic phase" (early April to the end of May). During this phase, the FrIAC crossed directly over the pole between 7 and 14 April. The VITA and Replay simulations transported the N2O anomaly intact during this crossing, in agreement with MLS, but unrealistic dispersion of the anomaly occurred in the GMI simulation due to excessive numerical mixing of the polar cap. The vortex associated with the FrIAC was apparently resistant to the weak vertical shear during the anticyclonic phase, and it thereby protected the embedded N2O anomaly from stretching. The vortex decayed in late May due to diabatic processes, leaving the N2O anomaly exposed to horizontal and vertical wind shears during the "shearing phase" (June to August). The observed lifetime of the FrIAC during this phase is consistent with timescales calculated from the ambient horizontal and vertical wind shear. Replay maintained the horizontal structure of the N2O anomaly similar to MLS well into August. Isentropic simulations using VITA also captured the horizontal structure of the FrIAC during this phase, but small-scale structures maintained by VITA are problematic and show that important mixing processes are absent from this single-level simulation.
Anthropogenic aerosols may have increased upper tropospheric humidity in the 20th century

Recent simulations of deep convection with a spectral microphysics cloud model show that an increase in aerosol concentration can have a significant effect on the nature of convection with more ice precipitation and less warm rain in polluted air. The cloud lifetime and the area covered by cloud anvils of deep convection are also larger for polluted air. Therefore, it is possible that the increase of anthropogenic aerosols in most of the 20th century has increased humidity and perhaps also cloudiness in the mid- to upper troposphere. Satellite data of upper tropospheric relative humidity in 1979–1997 and observed changes in cloudiness support this hypothesis. As changes in upper tropospheric humidity strongly affect longwave radiation, it is possible that anthropogenic aerosols have had a significant warming effect in addition to their other known effects on radiation.
Modeling sea-salt aerosol in a coupled climate and sectional microphysical model: mass, optical depth and number concentration

Sea-salt aerosol mass, optical depth, and number concentration over the global oceans have significant implications for aerosol direct and indirect climate effects. We model sea-salt aerosol in a coupled climate and sectional microphysical model, CAM/CARMA, with aerosol dynamics including sea-salt emission, gravitational sedimentation, dry deposition, wet scavenging, and hygroscopic growth. We aim to find an integrated sea-salt source function parameterization in the global climate model to simultaneously represent mass, optical depth, and number concentration. Each of these quantities is sensitive to a different part of the aerosol size distribution, which requires a size resolved microphysical model to treat properly. The CMS source function introduced in this research, based upon several earlier source functions, reproduces measurements of mass, optical depth and number concentration as well as the size distribution better than other source function choices we tried. However, as we note, it is also important to properly set the removal rate of the particles. The source function and removal rate are coupled in producing observed abundances. We find that sea salt mass and optical depth peak in the winter, when winds are highest. However, surprisingly, particle numbers and CCN concentrations peak in summer when rainfall is lowest. The quadratic dependence of sea-salt optical depth on wind speed, observed by some, is well represented in the model. We also find good agreement with the wind speed dependency of the number concentration at the measurement location and the regional scale. The work is the basis for further investigation of the effects of sea-salt aerosol on climate and atmospheric chemistry.
On the aerosol weekly cycle spatiotemporal variability over Europe

In this work, we focus on the spatial and temporal variability of the aerosol weekly cycle over Europe as these were recorded from TERRA MODIS and AQUA MODIS satellite instruments. Aerosol optical properties retrieved from MODIS TERRA (February 2000–February 2009) and AQUA (July 2002–December 2008) were used to produce an aerosol weekly cycle index. First, the general aerosol optical depth (AOD550 nm) weekly patterns were defined at a 1° × 1° resolution using the satellite-based index and six regions of interest were selected. To remove episodic dust transport events, two different aerosol flags, employing fine mode ratio (FMR550 nm) and AOD550 nm data, were applied diagnostically, showing that the observed weekly cycles over Europe are due to continental aerosols. A second spatial averaging method was then used for the investigation of the weekly variability and the statistical significance of the weekly cycle over each of the previously selected regions. Three major weekly cycle plumes are observed over Europe. A strong positive (higher values during midweek) weekly cycle plume appears over Central Europe, while a strong negative (higher values during weekend) weekly plume appears over the Iberian Peninsula and the North-eastern Europe. The temporal examination of the weekly cycles shows that in some areas there are seasonal differences in the sign of the weekly cycle. The aerosol weekly variability over different regions in Europe was examined in conjunction with the dominating synoptic wind patterns from the NCEP/NCAR reanalysis, showing that the seasonal weekly cycle plumes over regions situated in the eastern Europe and the Mediterranean Sea could be partly attributed to the westerly transport of continental aerosols.
Vertical profiles of droplet effective radius in shallow convective clouds

Conventional satellite retrievals can only provide information on cloud-top droplet effective radius (re). Given the fact that cloud ensembles in a satellite snapshot have different cloud-top heights, Rosenfeld and Lensky (1998) used the cloud-top height and the corresponding cloud-top re from the cloud ensembles in the snapshot to construct a profile of re representative of that in the individual clouds. This study investigates the robustness of this approach in shallow convective clouds based on results from large-eddy simulations (LES) for clean (aerosol mixing ratio Na = 25 mg−1), intermediate (Na = 100 mg−1), and polluted (Na = 2000 mg−1) conditions. The cloud-top height and the cloud-top re from the modeled cloud ensembles are used to form a constructed re profile, which is then compared to the in-cloud re profiles. For the polluted and intermediate cases where precipitation is negligible, the constructed re profiles represent the in-cloud re profiles fairly well with a low bias (about 10 %). The method used in Rosenfeld and Lensky (1998) is therefore validated for nonprecipitating shallow cumulus clouds. For the clean, drizzling case, the in-cloud re can be very large and highly variable, and quantitative profiling based on cloud-top re is less useful. The differences in re profiles between clean and polluted conditions derived in this manner are however, distinct. This study also investigates the subadiabatic characteristics of the simulated cumulus clouds to reveal the effect of mixing on re and its evolution. Results indicate that as polluted and moderately polluted clouds develop into their decaying stage, the subadiabatic fraction fad becomes smaller, representing a higher degree of mixing, and re becomes smaller (~10 %) and more variable. However, for the clean case, smaller fad corresponds to larger re (and larger re variability), reflecting the additional influence of droplet collision-coalescence and sedimentation on re. Finally, profiles of the vertically inhomogeneous clouds as simulated by the LES and those of the vertically homogeneous clouds are used as input to a radiative transfer model to study the effect of cloud vertical inhomogeneity on shortwave radiative forcing. For clouds that have the same liquid water path, re of a vertically homogeneous cloud must be about 76–90 % of the cloud-top re of the vertically inhomogeneous cloud in order for the two clouds to have the same shortwave radiative forcing.
Mesosphere-to-stratosphere descent of odd nitrogen in February–March 2009 after sudden stratospheric warming

We use the 3-D FinROSE chemistry transport model (CTM) and Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) observations to study connections between atmospheric dynamics and middle atmospheric NOx (NOx = NO + NO2) distribution. Two cases are considered in the northern polar regions: (1) descent of mesospheric NOx in February–March 2009 after a major sudden stratospheric warming (SSW) and, for comparison, (2) early 2007 when no NOx descent occurred. The model uses the European Centre for Medium-Range Weather Forecasts (ECMWF) operational data for winds and temperature, and we force NOx at the model upper altitude boundary (80 km) with ACE-FTS observations. We then compare the model results with ACE-FTS observations at lower altitudes. For the periods studied, geomagnetic indices are low, which indicates absence of local NOx production by particle precipitation. This gives us a good opportunity to study effects of atmospheric transport on polar NOx. The model results show no NOx descent in 2007, in agreement with ACE-FTS. In contrast, a large amount of NOx descends in February–March 2009 from the upper to lower mesosphere at latitudes larger than 60° N, i.e. inside the polar vortex. Both observations and model results suggest NOx increases of 150–200 ppb (i.e. by factor of 50) at 65 km due to the descent. However, the model underestimates the amount of NOx around 55 km by 40–60 ppb. According to the model results, chemical loss of NOx is insignificant during the descent period, i.e. polar NOx is mainly controlled by dynamics. The descent is terminated and the polar NOx amounts return to pre-descent levels in mid-March, when the polar vortex breaks. The break-up prevents the descending NOx from reaching the upper stratosphere, where it could participate in catalytic ozone destruction. Both ACE-FTS observations and FinROSE show a decrease of ozone of 20–30 % at 30–50 km from mid-February to mid-March. In the model, these ozone changes are not related to the descent but are due to solar activation of halogen and NOx chemistry.
Trends of HCl, ClONO2, and HF column abundances from ground-based FTIR measurements in Kiruna (Sweden) in comparison with KASIMA model calculations

Trends of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) total column abundances above Kiruna (Northern Sweden, 67.84° N, 20.41° E) derived from nearly 14 years (1996–2009) of measurement and model data are presented. The measurements have been performed with a Bruker 120 HR (later Bruker 125 HR) Fourier transform infrared (FTIR) spectrometer and the chemistry-transport model (CTM) used was KASIMA (KArlsruhe SImulation model of the Middle Atmosphere). The total column abundances of ClONO2 and HF calculated by KASIMA agree quite well with the FTIR measurements while KASIMA tends to underestimate the HCl columns. To calculate the long-term trends, a linear function combined with an annual cycle was fitted to the data using a least squares method. The precision of the resulting trends was estimated with the bootstrap resampling method. For HF, both model and measurements show a positive trend that seems to decrease in the last few years. This suggests a stabilisation of the HF total column abundance. Between 1996 and 2009, KASIMA simulates an increase of (+1.51±0.07) %/yr which exceeds the FTIR result of (+0.65±0.25) %/yr. The trends determined for HCl and ClONO2 are significantly negative over the time period considered here. This is expected because the emission of their precursors (chlorofluorocarbons and hydrochlorofluorocarbons) has been restricted in the Montreal Protocol in 1987 and its amendments and adjustments. The trend for ClONO2 from the FTIR measurements amounts to (−3.28±0.56) %/yr and the one for HCl to (−0.81±0.23) %/yr. KASIMA simulates a weaker decrease: For ClONO2, the result is (−0.90±0.10) %/yr and for HCl (−0.17±0.06) %/yr. Part of the difference between measurement and model data can be explained by sampling and the stronger annual cycle indicated by the measurements. There is a factor of about four between the trends of HCl and ClONO2 above Kiruna for both measurement and model data.
VOC reactivity and its effect on ozone production during the HaChi summer campaign

Measurements of ozone and its precursors conducted within the HaChi (Haze in China) project in summer 2009 were analyzed to characterize volatile organic compounds (VOCs) and their effects on ozone photochemical production at a suburban site in the North China Plain (NCP). Ozone episodes, during which running 8-h average ozone concentrations exceeding 80 ppbv lasted for more than 4 h, occurred on about two thirds of the observational days during the 5-week field campaign. This suggests continuous ozone exposure risks in this region in the summer. Average concentrations of nitrogen oxides (NOx) and VOCs are about 20 ppbv and 650 ppbC, respectively. On average, total VOC reactivity is dominated by anthropogenic VOCs. The contribution of biogenic VOCs to total ozone-forming potential, however, is also considerable in the daytime. Key species associated with ozone photochemical production are 2-butenes (18 %), isoprene (15 %), trimethylbenzenes (11 %), xylenes (8.5 %), 3-methylhexane (6 %), n-hexane (5 %) and toluene (4.5 %). Formation of ozone is found to be NOx-limited as indicated by measured VOCs/NOx ratios and further confirmed by a sensitivity study using a photochemical box model NCAR_MM. The Model simulation suggests that ozone production is also sensitive to changes in VOC reactivity under the NOx-limited regime, although this sensitivity depends strongly on how much NOx is present.
Impact of nitrous acid chemistry on air quality modeling results over the Pearl River Delta region

The impact of nitrous acid chemistry on regional ozone and particulate matter in Pearl River Delta region was investigated using the Community Mutilscale Air Quality modeling system and the CB05 mechanism. Model simulations were conducted for a ten-day period in October 2004. Compared with available observed data, the model performance for NOx, SO2, PM10, and sulfate is reasonably good; however, predictions of HONO are an order of magnitude lower than observed data. The CB05 mechanism contains several homogenous reactions related to nitrous acid. To improve the model performance for nitrous acid, direct emissions, two heterogeneous reactions, and two surface photolysis reactions were incorporated into the model. The inclusion of the additional formation pathways significantly improved simulated nitrous acid compared with observed data. The addition of nitrous acid sources enhance daily maximum 8-h ozone by up to 6 ppb V (8 %) and daily mean PM2.5 by up to 17 μg m−3 (12 %). They also affected ozone control strategy in Pearl River Delta region.
Decreases in elemental carbon and fine particle mass in the United States

Observations at national parks and other remote sites show that average elemental carbon and fine particle mass concentrations in the United States both decreased by over 25 % between 1990 and 2004. Percentage decreases in elemental carbon were much larger in winter than in summer. These data suggest that emissions controls have been effective in reducing particulate concentrations not only in polluted areas but also across the United States. Despite the reduction in elemental carbon, the simultaneous decrease in non-absorbing particles implies that the overall radiative forcing from these changes was toward warming. The use of a 2005 instead of 1990 as a baseline for climate-relevant emissions from the United States would imply a significantly lower baseline for aerosol emissions. The use of older data will overestimate the possibility for future reductions in warming due to black carbon controls.